Float-stacked graphene-PMMA laminate.

Semi-infinite single-atom-thick graphene is an ideal reinforcing material that can simultaneously improve the mechanical, electrical, and thermal properties of matrix. Here, we present a float-stacking strategy to accurately align the monolayer graphene reinforcement in polymer matrix. We float graphene-poly(methylmethacrylate) (PMMA) membrane (GPM) at the water-air interface, and wind-up layer-by-layer by roller. During the stacking process, the inherent water meniscus continuously induces web tension of the GPM, suppressing wrinkle and folding generation. Moreover, rolling-up and hot-rolling mill process above the glass transition temperature of PMMA induces conformal contact between each layer. This allows for pre-tension of the composite, maximizing its reinforcing efficiency. The number and spacing of the embedded graphene fillers are precisely controlled. Notably, we accurately align 100 layers of monolayer graphene in a PMMA matrix with the same intervals to achieve a specific strength of about 118.5 MPa g-1 cm3, which is higher than that of lightweight Al alloy, and a thermal conductivity of about 4.00 W m-1 K-1, which is increased by about 2,000 %, compared to the PMMA film.

Layer-engineered large-area exfoliation of graphene.

The competition between quality and productivity has been a major issue for large-scale applications of two-dimensional materials (2DMs). Until now, the top-down mechanical cleavage method has guaranteed pure perfect 2DMs, but it has been considered a poor option in terms of manufacturing. Here, we present a layer-engineered exfoliation technique for graphene that not only allows us to obtain large-size graphene, up to a millimeter size, but also allows selective thickness control. A thin metal film evaporated on graphite induces tensile stress such that spalling occurs, resulting in exfoliation of graphene, where the number of exfoliated layers is adjusted by using different metal films. Detailed spectroscopy and electron transport measurement analysis greatly support our proposed spalling mechanism and fine quality of exfoliated graphene. Our layer-engineered exfoliation technique can pave the way for the development of a manufacturing-scale process for graphene and other 2DMs in electronics and optoelectronics.